Advancing the US Department of Energy’s Priority Research Opportunities for Carbon Neutral Hydrogen Technologies, this project develops high-precision approaches to synthesize and study nanoscale metal hydrides. Multiple BES Hydrogen Roundtables have identified these materials as pivotal to progress in hydrogen storage, high-capacity battery components, and electrocatalysts for water splitting and CO₂ reduction. Research focuses on creating atomically precise metal hydride nanoclusters and examining how their structures relate to performance. Efforts include defining hydride binding behavior, clarifying the nature of surface hydride species, and integrating structural and electrochemical insights to establish accurate structure-property correlations. Impact centers on strengthening the scientific foundation for safer, more efficient carbon-neutral hydrogen technologies. Outcomes contribute to national goals for clean energy, resilient infrastructure, and reduced emissions by advancing materials that can support next-generation hydrogen systems and related energy applications.